Ligand-Directed Self-Assembly of Organic-Semiconductor/Quantum-Dot Blend Films Enables Efficient Triplet Exciton-Photon Conversion
Year: 2024
Type: article
Abstract: Blends comprising organic semiconductors and inorganic quantum dots (QDs) are relevant for many optoelectronic applications and devices. However, the individual components in organic-QD blends have a strong tendency to aggregate and phase-separate during film processing, compromising both their structural and electronic properties. Here, we demonstrate a QD surface engineering approach using electronically active, highly soluble semiconductor ligands that are matched to the organic semiconductor host material to achieve well-dispersed inorganic-organic blend films, as characterized by X-ray and neutron scattering, and electron microscopies. This approach preserves the electronic properties of the organic and QD phases and also creates an optimized interface between them. We exemplify this in two emerging applications, singlet-fission-based photon multiplication (SF-PM) and triplet-triplet annihilation-based photon upconversion (TTA-UC). Steady-state and time-resolved optical spectroscopy shows that triplet excitons can be transferred with near unity efficiently across the organic-inorganic interface, while the organic films maintain efficient SF (190% yield) in the organic phase. By changing the relative energy between organic and inorganic components, yellow upconverted emission is observed upon 790 nm NIR excitation. Overall, we provide a highly versatile approach to overcome longstanding challenges in the blending of organic semiconductors with QDs that have relevance for many optical and optoelectronic applications.
DOI: 10.1021/jacs.4c00125
Authors: Victor Gray, Daniel T. W. Toolan, Simon Dowland, Jesse R. Allardice, Michael P. Weir, Zhilong Zhang, James Xiao, Anastasia Klimash, Jurjen F. Winkel, Emma K. Holland, Garrett M. Fregoso, John E. Anthony, Hugo Bronstein, Richard Friend, Anthony J. Ryan, Richard A. L. Jones, Neil C. Greenham, Akshay Rao
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $4,500
Awards: Controlling Wavefunction Overlap for Triplet Energy Transfer in Organic/Nanocrystal Quantum Dots Hybrids, DMREF: Collaborative Research: Organic Semiconductors by Computationally-Accelerated Refinement (OSCAR), Making Dark Triplets From Singlet Fission Bright - Improving Solar Cell Efficiencies, Controlling Wavefunction Overlap for Triplet Energy Transfer in Organic/Nanocrystal Quantum Dots Hybrids, G434337789, Photon Management for Solar Energy Harvesting with Hybrid Excitonics, G5922959832, G712881263, G7358480839, EPSRC Centre for Doctoral Training in Sustainable and Functional Nano, Rational design of manufacturing processes for next generation optoelectronically active nanocomposite films and coatings, G7756600463, G7899748958, Manufacturing Organic-Inorganic Nanoparticle Composites with Nanoscale Precision via Directed Self-Assembly
OpenAlex ID: W4392597641